JP3909791B2 - Transfer method of transparent conductive film - Google Patents

Transfer method of transparent conductive film Download PDF

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Publication number
JP3909791B2
JP3909791B2 JP11031099A JP11031099A JP3909791B2 JP 3909791 B2 JP3909791 B2 JP 3909791B2 JP 11031099 A JP11031099 A JP 11031099A JP 11031099 A JP11031099 A JP 11031099A JP 3909791 B2 JP3909791 B2 JP 3909791B2
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Prior art keywords
transparent conductive
conductive film
substrate
layer
adhesive layer
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JP2000306441A (en
Inventor
一郎 別宮
忠宏 古川
明良 村上
和己 新井
尚 佐藤
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Kyodo Printing Co Ltd
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Kyodo Printing Co Ltd
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Priority to JP11031099A priority Critical patent/JP3909791B2/en
Priority to US09/548,952 priority patent/US6413693B1/en
Priority to EP00303238A priority patent/EP1046945B1/en
Priority to DE60040361T priority patent/DE60040361D1/en
Priority to TW089107242A priority patent/TW514607B/en
Priority to KR10-2000-0020243A priority patent/KR100382824B1/en
Publication of JP2000306441A publication Critical patent/JP2000306441A/en
Priority to US10/027,289 priority patent/US6830864B2/en
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    • G—PHYSICS
    • G02—OPTICS
    • G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
    • G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
    • G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour 
    • G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour  based on liquid crystals, e.g. single liquid crystal display cells
    • G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
    • G02F1/1333—Constructional arrangements; Manufacturing methods
    • G02F1/1343—Electrodes
    • G02F1/13439—Electrodes characterised by their electrical, optical, physical properties; materials therefor; method of making
    • G—PHYSICS
    • G02—OPTICS
    • G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
    • G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
    • G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour 
    • G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour  based on liquid crystals, e.g. single liquid crystal display cells
    • G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
    • G02F1/1333—Constructional arrangements; Manufacturing methods
    • G02F1/1335—Structural association of cells with optical devices, e.g. polarisers or reflectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B13/00—Apparatus or processes specially adapted for manufacturing conductors or cables

Description

【０００１】
【発明の属する技術分野】
この発明は、プラスチック材料からなるシート基材の一面に、転写によって透明導電膜を形成する技術であり、転写すべき透明導電膜を、プラスチック材料に比べて耐熱性にすぐれた基板側に形成しておく転写技術に関する。
【０００２】
【発明の背景】
この種の転写技術は、液晶表示装置などの光学的な表示装置のための電極あるいは配線となる透明導電膜を形成する技術の一つとして知られている。この転写による技術は、基本的に、一時的に透明導電膜を支持する仮の基板上に、剥離層を介して透明導電膜を形成しておき、その透明導電膜を接着剤の層を介して別のシート基材に転写するという方法である。その基本については、たとえば特開平２−１７４０１１の公報が示している。なお、接着剤層については、一般に、仮の基板の透明導電膜上に形成するが、場合によっては、別のシート基材の側に形成しておくこともできる。
【０００３】
転写すべき透明導電膜としては、ＩＴＯ（インジウム−チン−オキサイド）やＳｎＯ2などの金属酸化物を用いるが、それらの材料は、高温で成膜するほど低抵抗を示す。実用上、たとえば１５０℃以上の基板温度で比抵抗３．０×１０‐4Ωｃｍ以下の特性が望まれる。そこで、その上に透明導電膜を形成する仮の基板としては、最終的に透明導電膜を支持する別のシート基材に比べて耐熱性にすぐれたものを選択すべきである。特に、別のシート基材として、プラスチック材料を用いる場合には、それが肝要である。その点から、特開平１１−２４０８１号の公報は、剥離層の材料としてポリイミド樹脂を用い、しかも、仮の基板として、ポリイミド樹脂を有効に塗膜化するため、分子内に弗素原子および珪素原子を含まず、かつ剥離層のポリイミドの焼成温度を超えるガラス転移温度をもつ耐熱性ポリマーを用いる技術を示している。
【０００４】
発明者らは、そうした転写によって透明導電膜を形成する技術について、いろいろと実験し検討したところ、仮の基板の側から透明導電膜を別のシート基材の側に転写する際、その透明導電膜にクラックが発生するおそれがあることに着目した。その原因を探ったところ、透明導電膜が薄く比較的にもろい性質をもち、それが転写時に加わる外力に耐えきれないことに起因していることが判明した。外力の主因は、透明導電膜をシート基材の側に接着するための接着剤の硬化収縮に伴う応力であり、それが転写時に仮の基板を引き剥がす際に透明導電膜に作用することになる。また、転写後にそうした応力が残ると、高温、高湿等のストレスがかかった場合にクラックが発生しやすくなる。このような接着剤の側から加わる応力に対し、透明導電膜を保護するという考え方は、前記した公報を含め今までは何も考慮されていなかった。そして特に、そうした応力に起因する問題は、耐熱性の仮の基板として、セラミックス、ガラス、金属（４２アロイ、銅合金等の熱膨張の小さい金属材料が好適である）の単体、あるいはそれらの複数を積層し複合したものなど、プラスチック材料であるシート基材に比べて大きな剛性をもつものを用いるときに顕著である。また、これらの仮の基板は、パターン形成を前提にすると、温度や湿度に対する寸法安定性が重要であり、プラスチック材料は望ましい材料ではない。
【０００５】
【発明の解決すべき課題】
したがって、この発明は、転写時の外力から透明導電膜を有効に保護する技術を提供することを第１の目的とする。
また、この発明は、外力の主因となる接着剤の層の厚さを有効に制御することができる技術を提供することを他の目的とする。
【０００６】
【課題を解決するための手段】
この発明では、耐熱性にすぐれた基板の側に予め形成した透明導電膜を、プラスチック材料からなるシート基材の側に転写するに際し、転写すべき透明導電膜を、耐熱性の基板上、転写時に剥離部分となる剥離層と、前記したクラックの発生から保護するための保護膜とでサンドイッチ状にはさみ込んだ形態にする。透明導電膜は、転写時、剥離層と保護膜とによって保護されているため、特に接着剤層の側の保護膜が前記した外力を吸収あるいは緩衝するように作用し、クラックの発生を有効に防ぐことができる。
【０００７】
透明導電膜をサンドイッチ状にはさむ一方の剥離層としては、透明導電膜の材料であるＩＴＯ等を高温で成膜可能なだけの耐熱性、そうしたＩＴＯ等とのしっかりした密着性、透明導電膜をパターニングする際のエッチングプロセス等に対する耐性、さらには、仮の基板との適度な密着性（剥離するまでにしっかりと仮の基板に密着し、しかも、他層にダメージを与えずに剥離可能であるような密着性であり、たとえば、９０°剥離で数ｇ〜１００ｇ／ｃｍ程度の引き剥がし力が必要なだけの密着性）をもつことが必要である。この剥離層として好適な材料はポリイミドである。前記した特開平１１−２４０８１号の公報の７ページの比較例１では、ポリイミド膜−ガラス基板の場合、剥離しにくいという記載があるが、実験によれば、仮の基板がガラスであっても特別な処理を行うことなくポリイミド膜は剥離可能である。しかし、ポリイミドも種類によってガラスとの密着性を異にする。ピロメリット酸無水物と４，４’−ジアミノジフェニルエーテルから合成される第１のものは、表面にＳｉＯ2がコートされたガラスとの密着性はそれほど良くなく、剥離層の材料として適している。それに対し、ベンゾフェノンテトラカルボン酸無水物、あるいはピロメリット酸無水物と３，３’−ジアミノジフェニルスルホンから合成される第２のポリイミドは、第１のものよりもガラスとの密着性が良い。しかも、ポリイミドとガラスとの密着性はベークをすると良くなり、時間の経過とともに次第に低下し、一定のところで変化しなくなる。しかし、そのように密着性が低下したものを再びベークすると、密着性は元に戻る。第１のポリイミドはベーク直後でもガラスから剥離することができるが、数日すると水洗でも剥がれてしまうほど密着性が低下する（９０°剥離で１ｇ／ｃｍ未満）。それに対し、第２のポリイミドはベーク直後ではガラスから剥がすことができないが、時間が経過すれば剥がすことができるようになる。こうしたポリイミドの密着性の変化は、ポリイミドの吸湿が原因していると考えられる。したがって、ポリイミドのそうした特性を考慮しつつ、ポリイミドを剥離層として用いることができる。また、たとえば密着性の良くない第１のポリイミドにシランカップリング剤を添加することによって、ガラスとの密着性を最適化することができる。
【０００８】
一方、透明導電膜をサンドイッチ状にはさむ他方の保護膜は、剥離層と相俟って透明導電膜を保護するための膜であり、アルキッド、アクリル、ウレタン等の有機系の樹脂のほか、無機系、あるいは無機系と有機系とのハイブリッド樹脂などを用いることできる。無機系の材料として、たとえばテトラアルコキシシランのアルコール溶液（コーティング溶液）があり、より厚く塗布する際には、これに有機成分を入れたコーティング溶液もある（たとえば、商品名セラメートＣ−５３３、ＺＲＳ−５ＰＨ／触媒化成）。剥離層が０．１〜２μｍ、透明導電膜が０．１〜０．４μｍの厚さに対し、保護膜は０．５〜２μｍの厚さであり、保護特性の点からすると、その硬さを鉛筆硬度（ＪＩＳ Ｋ５４０１）がＨ以上、好ましくは２Ｈ以上に設定するのが良い。また、この保護膜の上にカラー表示のためのカラーフィルタ層を形成するときには、剥離層の除去に対しカラーフィルタ層および接着剤層を保護する機能をもたせるようにもすべきである。
【０００９】
さらに、透明導電膜としては、前記したＩＴＯやＳｎＯ ２ などの金属酸化物を用いることができ、特には、透明性および比抵抗などの特性面ですぐれたＩＴＯが好ましい。このＩＴＯなどは、スパッタ、イオンプレーティングあるいは電子ビーム蒸着などの公知の方法によって形成することができる。また、耐熱性の仮の基板としては、セラミックス、ガラス、金属の単体か、それらが複合された基板を広く適用することができるが、特にはガラス基板が好ましい。ガラスは耐熱性にすぐれるだけでなく、その上に透明導電膜やカラーフィルタ層などを正確に位置合わせしつつ形成することができるからである。そして、ガラスは、前記したように、剥離層の材料であるポリイミドとの関係からも好適な材料である。
【００１０】
次に、透明導電膜をシート基材の側に接着するための接着剤層としては、熱をかけずに硬化する紫外線硬化型のものが好ましい。その中でもカチオン重合型のもの、たとえば、エポキシ系の紫外線硬化型接着剤が最適である。塗布の厚さは、２〜２０μｍ程度であり、充分な接着強度を得ることができ、透過率を失わない薄さをもつ値に設定する。こうした接着剤層は、ラミネート時の押圧条件により膜厚分布に差が生じたり、脇から接着剤がはみ出したりする。そのため、接着剤層の部分に、その接着剤層の厚さを制御するためのスペーサ手段を設けるようにするのが良い。スペーサ手段としては、接着剤層の中に混入したスペーサ粒子、あるいは保護膜の上に形成したスペーサパターンなどを用いることができる。
【００１１】
なお、プラスチック材料からなるシート基材は、シート（枚葉）、ロールのいずれの形態でも用いることができ、好ましい厚さは１００〜７００μｍの範囲である。したがって、ここでいうシート基材は、いわゆるフィルムやシートを含むシート状の部材を包含する概念である。材料であるプラスチックとしては、ポリエーテルスルホン、ポリエステル、ポリカーボネート、塩化ビニール、ナイロン、ポリアリレート、アクリル、ポリイミド等を適用することができる。
【００１２】
【実施例】
以下、添付の図面に示す実施例を参照しながら、この発明の内容をさらに具体的に説明する。
まず、図１に示すように、洗浄したガラス基板１０を用意し、その一面に剥離層としての透明なポリイミド層２０を塗布によって形成する。ガラス基板１０の厚さは０．７〜１．１ｍｍ程度であり、全体として剛性をもっている。このガラス基板１０は、その表面に転写すべき透明導電膜などを支持する基板であるため、良好な表面平滑性、たとえば暗室下５０００Ｌｕｘの明るさの反射光で目視により観察した時にキズや突起等が見えない程度の表面平滑性（基板表面の外観規格）をもっていることが望ましい。また、ポリイミド層２０は、前記した第１のポリイミドに固形分比で０．１％のシランカップリング剤を添加したものであり、その厚さが０．１〜２μｍである。勿論、このポリイミド層２０については、塗布した後、加熱処理により硬化させる。ガラス基板１０は、ポリイミド硬化のための加熱処理に充分に耐えうることは勿論である。
【００１３】
次に、図２に示すように、そうしたガラス基板１０のポリイミド層２０上に、ＩＴＯ膜を成膜した後、それをパターニングすることによって、透明導電膜３０を形成する。ＩＴＯ膜の成膜に当たってはガラス基板１０の温度を１５０℃以上とし、前記したような比抵抗の低い膜を得る。そして、図３に示すように、ガラス基板１０上の透明導電膜３０を被うように、アクリル系の保護膜４０を１〜２μｍの厚さに形成する。
【００１４】
この後、図４に示すように、保護膜４０の上にイエロー、マゼンタ、シアンの色パターン５０Ｙ，５０Ｍ，５０Ｃを含むカラーフィルタ層５０をフォトリソグラフィ法によって形成する。色パターン５０Ｙ，５０Ｍ，５０Ｃの材料として、染料あるいは顔料などの着色剤をポリイミド樹脂溶液に溶解あるいは分散させた公知の塗布材料を用いることができる（たとえば、特開平１０−１７０７１６号）。各色パターンはストライプ形状であり、その幅は５０〜２００μｍであり、隣り合う色パターンの間の距離は５〜２０μｍである。また、カラーフィルタ層５０は、反射型のものであり、その厚さが０．２〜２μｍである。この際、カラーフィルタ層５０の各色パターン５０Ｙ，５０Ｍ，５０ＣおよびパターニングしたＩＴＯ膜は、寸法安定性にすぐれたガラス基板１０上で位置合わせを行っているので、パターニングや位置合わせの上で何ら問題が起こらない。
【００１５】
さらに、図５に示すように、カラーフィルタ層５０の上を全体的に被うように、接着剤層６０を塗布によって形成する。接着剤層６０としては、紫外線硬化型であり、カチオン重合型のエポキシ系の紫外線硬化型接着剤（旭電化工業株式会社製のＵＶ硬化樹脂ＫＲ５００）を用いる。塗布の厚さは、２〜２０μｍ程度であり、充分な接着強度を得ることができ、透過率を失わない薄さをもつ値に設定する。このとき、接着剤層６０の中に、スペーサ手段としてスペーサ粒子、たとえばベンゾグアナミンの４μｍ球形粒子（図示しない）を混入する。スペーサ粒子は、塗布すべき材料の中に予め添加しておき、基板１０への塗布を行う。この際、接着剤は液状であり、スペーサ粒子の大きさよりやや厚めに塗膜の厚さをコントロールすることが望ましい。この状態でガラス基板１０とプラスチックシートであるシート基材８０をラミネートすると、膜厚が全面均一の接着剤層６０を得ることができる。なお、スペーサ粒子の混入量としては、接着剤層６０を形成した後で、面内分布量が４０個／ｍｍ2程度となるよう調整するのが好ましい。ここで、接着剤層６０のエポキシ樹脂は、光硬化によってたとえば数％程度の体積収縮を生じるが、スペーサ粒子はそうした変化が生じにくい。そのため、接着剤層６０の体積収縮に伴ってスペーサ粒子の部分に不都合な変形や応力が生じ、ＩＴＯ膜にクラックが生じることがある。これを避けるため、スペーサ粒子の粒子径は所定以下の大きさにすべきであり、たとえば５．５μｍ以下に設定するのが好ましい。スペーサ手段としては、スペーサ粒子のほか、図６に示すように、カラーフィルタ層５０の各色パターン５０Ｙ，５０Ｍ，５０Ｃの間（この部分は、透明導電膜３０のパターンがない部分でもある）に、島状あるいはストライプ状にパターニングしたスペーサパターン７０を用いることもできる。スペーサパターン７０は、不都合な変形や応力によって透明導電膜３０に損傷を与えるようなことがない。また、スペーサパターン７０は、黒色の色材を混入したポリイミド樹脂を利用して形成することができる。そうすれば、液晶表示をするとき、表示のコントラストを向上させるというメリットをも得る。
【００１６】
この後、図７に示すように、接着剤層６０の側に、ポリエーテルスルホン基板からなるシート基材８０（厚さが１００〜７００μｍ）を配置し、透明導電膜３０およびカラーフィルタ層５０などをガラス基板１０側からシート基材８０側に転写する。この転写処理に際しては、シート基材８０側から紫外線を照射するが、併せて、照射に伴う接着剤層６０の側（硬化対象物）の温度上昇を積極的に抑え、できるだけ常温に近い温度にする。この転写時、特にダメージを受けやすい透明導電膜３０は、剥離層としてのポリイミド膜２０と保護膜４０との間にサンドイッチされているため、接着剤層６０の硬化および転写に伴う外力から有効に保護される。
【００１７】
転写後、剥離層としてのポリイミド層２０を除去する。それは、透明導電膜３０と液晶表示のためのドライバーＩＣとの電気的な接続を可能とするためでもあり、液晶駆動のための実効電圧の向上を図るためでもある。ポリイミド層２０の除去については、ヒドラジン−エチレンジアミンを用いた湿式エッチングを用いる。この際、前記保護膜４０は、このエッチャントから接着剤層６０、カラーフィルタ層５０を保護する。
【図面の簡単な説明】
【図１】剥離層を形成したガラス基板を示す断面図である。
【図２】ガラス基板上に透明導電膜を形成した状態を示す断面図である。
【図３】透明導電膜のパターンの上に保護膜を形成した状態を示す断面図である。
【図４】保護膜の上にカラーフィルタ層を形成した状態を示す断面図である。
【図５】カラーフィルタ層の上に接着剤層を塗布した状態を示す断面図である。
【図６】スペーサパターンを利用した場合の断面図である。
【図７】転写の際の状態を示す断面図である。
【符号の説明】
１０ ガラス基板
２０ ポリイミド層（剥離層）
３０ 透明導電膜
４０ 保護膜
５０ カラーフィルタ層
６０ 接着剤層
７０ スペーサパターン
８０ シート基材[0001]
BACKGROUND OF THE INVENTION
This invention is a technique for forming a transparent conductive film on one surface of a sheet base material made of a plastic material by transfer, and the transparent conductive film to be transferred is formed on the substrate side, which is superior in heat resistance compared to the plastic material. It relates to transfer technology.
[0002]
BACKGROUND OF THE INVENTION
This type of transfer technique is known as one of the techniques for forming a transparent conductive film to be an electrode or wiring for an optical display device such as a liquid crystal display device. In this transfer technique, basically, a transparent conductive film is formed on a temporary substrate that temporarily supports the transparent conductive film via a release layer, and the transparent conductive film is then passed through an adhesive layer. Transfer to another sheet base material. The basics are disclosed in, for example, Japanese Patent Laid-Open No. 2-174011. The adhesive layer is generally formed on the transparent conductive film of the temporary substrate, but may be formed on the side of another sheet base material depending on the case.
[0003]
As the transparent conductive film to be transferred, a metal oxide such as ITO (indium-tin-oxide) or SnO2 is used, and these materials exhibit lower resistance as the film is formed at a higher temperature. Practically, for example, characteristics with a specific resistance of 3.0 × 10 −4 Ωcm or less at a substrate temperature of 150 ° C. or higher are desired. Therefore, as the temporary substrate on which the transparent conductive film is formed, a substrate having excellent heat resistance as compared with another sheet base material that finally supports the transparent conductive film should be selected. In particular, when a plastic material is used as another sheet base material, it is essential. In view of this, Japanese Patent Application Laid-Open No. 11-24081 uses a polyimide resin as a material for the release layer, and in order to effectively form a polyimide resin film as a temporary substrate, And a technique using a heat-resistant polymer having a glass transition temperature exceeding the firing temperature of the polyimide of the release layer.
[0004]
The inventors have experimented and studied various techniques for forming a transparent conductive film by such transfer. When transferring the transparent conductive film from the temporary substrate side to another sheet base material side, the transparent conductive film is formed. We paid attention to the possibility of cracks in the film. As a result of investigating the cause, it was found that the transparent conductive film is thin and has a relatively fragile property, which cannot withstand the external force applied during transfer. The main cause of external force is the stress accompanying the curing shrinkage of the adhesive for adhering the transparent conductive film to the sheet substrate side, and it acts on the transparent conductive film when peeling off the temporary substrate at the time of transfer Become. If such stress remains after transfer, cracks are likely to occur when stress such as high temperature and high humidity is applied. The concept of protecting the transparent conductive film against the stress applied from the adhesive side has not been considered until now, including the above-mentioned gazette. In particular, the problem caused by such stress is that, as a heat-resistant temporary substrate, ceramic, glass, metal (a metal material having a small thermal expansion such as 42 alloy or copper alloy is preferable), or a plurality of them. This is conspicuous when a material having a larger rigidity than a sheet base material that is a plastic material, such as a composite material obtained by laminating and composites. In addition, when these temporary substrates are premised on pattern formation, dimensional stability with respect to temperature and humidity is important, and plastic materials are not desirable materials.
[0005]
Problems to be Solved by the Invention
Accordingly, a first object of the present invention is to provide a technique for effectively protecting a transparent conductive film from an external force during transfer.
Another object of the present invention is to provide a technique capable of effectively controlling the thickness of an adhesive layer that is a main cause of external force.
[0006]
[Means for Solving the Problems]
In this invention, when transferring the transparent conductive film previously formed on the side of the substrate having excellent heat resistance to the side of the sheet base material made of plastic material, the transparent conductive film to be transferred is transferred onto the heat resistant substrate. A sandwich layer is sometimes formed between a release layer that sometimes becomes a release portion and a protective film for protecting against the occurrence of cracks. Since the transparent conductive film is protected by the peeling layer and the protective film at the time of transfer, the protective film on the side of the adhesive layer acts so as to absorb or buffer the external force described above, effectively generating cracks. Can be prevented.
[0007]
As the peeling layer that sandwiches the transparent conductive film in a sandwich shape, heat resistance that allows ITO, which is a material of the transparent conductive film, to be formed at a high temperature, firm adhesion with such ITO, etc. Resistance to etching process during patterning, and appropriate adhesion to temporary substrate (adheres firmly to temporary substrate before peeling, and can be removed without damaging other layers) For example, it is necessary to have adhesiveness that requires a peeling force of about several g to 100 g / cm at 90 ° peeling. A suitable material for the release layer is polyimide. In Comparative Example 1 on page 7 of the above-mentioned Japanese Patent Application Laid-Open No. 11-24081, there is a description that it is difficult to peel in the case of a polyimide film-glass substrate, but according to experiments, even if the temporary substrate is glass, The polyimide film can be peeled off without any special treatment. However, polyimide also has different adhesion to glass depending on the type. The first compound synthesized from pyromellitic anhydride and 4,4′-diaminodiphenyl ether does not have very good adhesion with glass whose surface is coated with SiO2, and is suitable as a material for the release layer. On the other hand, the second polyimide synthesized from benzophenone tetracarboxylic anhydride or pyromellitic anhydride and 3,3′-diaminodiphenyl sulfone has better adhesion to glass than the first. Moreover, the adhesion between the polyimide and the glass is improved by baking, and gradually decreases with the passage of time, and does not change at a certain point. However, when the adhesive having such a lowered adhesiveness is baked again, the adhesiveness is restored. The first polyimide can be peeled off from the glass even immediately after baking, but after a few days, the adhesiveness decreases so as to be peeled off even after washing with water (less than 1 g / cm at 90 ° peeling). On the other hand, the second polyimide cannot be peeled off from the glass immediately after baking, but can be peeled off after a lapse of time. Such a change in adhesion of polyimide is considered to be caused by moisture absorption of polyimide. Therefore, it is possible to use polyimide as a release layer while considering such characteristics of polyimide. Further, for example, by adding a silane coupling agent to the first polyimide having poor adhesion, the adhesion with glass can be optimized.
[0008]
On the other hand, the other protective film sandwiching the transparent conductive film is a film for protecting the transparent conductive film in combination with the release layer. In addition to organic resins such as alkyd, acrylic and urethane, inorganic Or a hybrid resin of inorganic type and organic type can be used. As an inorganic material, for example, there is an alcohol solution (coating solution) of tetraalkoxysilane, and when applying thicker, there is also a coating solution in which an organic component is added (for example, trade names Ceramate C-533, ZRS). -5PH / catalyst conversion). The protective layer has a thickness of 0.5 to 2 μm, whereas the peelable layer has a thickness of 0.1 to 2 μm and the transparent conductive film has a thickness of 0.1 to 0.4 μm. Is set to a pencil hardness (JIS K5401) of H or higher, preferably 2H or higher. Further, when a color filter layer for color display is formed on the protective film, it should have a function of protecting the color filter layer and the adhesive layer against the removal of the release layer.
[0009]
Furthermore, as the transparent conductive film, the above-described metal oxides such as ITO and SnO 2 can be used. In particular, ITO excellent in characteristics such as transparency and specific resistance is preferable. The ITO or the like can be formed by a known method such as sputtering, ion plating, or electron beam evaporation. In addition, as the heat-resistant temporary substrate, ceramics, glass, a single metal, or a substrate in which they are combined can be widely applied, and a glass substrate is particularly preferable. This is because glass is not only excellent in heat resistance, but can be formed while accurately aligning a transparent conductive film, a color filter layer, and the like thereon. And glass is a suitable material also from the relationship with the polyimide which is a material of a peeling layer as mentioned above.
[0010]
Next, the adhesive layer for adhering the transparent conductive film to the sheet substrate side is preferably an ultraviolet curable type that cures without applying heat. Among them, a cationic polymerization type, for example, an epoxy ultraviolet curing adhesive is most suitable. The thickness of the coating is about 2 to 20 μm, and can be set to a value having such a thickness that sufficient adhesive strength can be obtained and the transmittance is not lost. Such an adhesive layer has a difference in film thickness distribution depending on pressing conditions during lamination, or the adhesive protrudes from the side. Therefore, it is preferable to provide spacer means for controlling the thickness of the adhesive layer in the adhesive layer portion. As the spacer means, spacer particles mixed in the adhesive layer or a spacer pattern formed on the protective film can be used.
[0011]
In addition, the sheet | seat base material which consists of plastic materials can be used with any form of a sheet | seat (sheet | leaf) and a roll, and preferable thickness is the range of 100-700 micrometers. Therefore, the sheet base material here is a concept including a sheet-like member including a so-called film or sheet. As the plastic material, polyethersulfone, polyester, polycarbonate, vinyl chloride, nylon, polyarylate, acrylic, polyimide, and the like can be applied.
[0012]
【Example】
Hereinafter, the content of the present invention will be described more specifically with reference to the embodiments shown in the accompanying drawings.
First, as shown in FIG. 1, a cleaned glass substrate 10 is prepared, and a transparent polyimide layer 20 as a release layer is formed on one surface thereof by coating. The thickness of the glass substrate 10 is about 0.7 to 1.1 mm, and has rigidity as a whole. Since this glass substrate 10 is a substrate that supports a transparent conductive film to be transferred on its surface, it has good surface smoothness, such as scratches and protrusions when visually observed with reflected light having a brightness of 5000 Lux under a dark room. It is desirable to have a surface smoothness (appearance standard of the substrate surface) that cannot be seen. In addition, the polyimide layer 20 is obtained by adding a silane coupling agent of 0.1% in terms of solid content to the first polyimide, and has a thickness of 0.1 to 2 μm. Of course, the polyimide layer 20 is applied and then cured by heat treatment. Of course, the glass substrate 10 can sufficiently withstand the heat treatment for curing the polyimide.
[0013]
Next, as shown in FIG. 2, after forming an ITO film on the polyimide layer 20 of the glass substrate 10, a transparent conductive film 30 is formed by patterning the ITO film. In forming the ITO film, the temperature of the glass substrate 10 is set to 150 ° C. or higher to obtain a film having a low specific resistance as described above. And as shown in FIG. 3, the acrylic protective film 40 is formed in thickness of 1-2 micrometers so that the transparent conductive film 30 on the glass substrate 10 may be covered.
[0014]
Thereafter, as shown in FIG. 4, a color filter layer 50 including yellow, magenta, and cyan color patterns 50Y, 50M, and 50C is formed on the protective film 40 by photolithography. As a material for the color patterns 50Y, 50M, and 50C, a known coating material in which a colorant such as a dye or a pigment is dissolved or dispersed in a polyimide resin solution can be used (for example, JP-A-10-170716). Each color pattern has a stripe shape, the width is 50 to 200 μm, and the distance between adjacent color patterns is 5 to 20 μm. The color filter layer 50 is of a reflective type and has a thickness of 0.2 to 2 μm. At this time, the color patterns 50Y, 50M, and 50C of the color filter layer 50 and the patterned ITO film are aligned on the glass substrate 10 having excellent dimensional stability, so there is no problem in patterning or alignment. Does not happen.
[0015]
Further, as shown in FIG. 5, an adhesive layer 60 is formed by coating so as to cover the color filter layer 50 as a whole. As the adhesive layer 60, an ultraviolet curable epoxy-type ultraviolet curable adhesive (UV curable resin KR500 manufactured by Asahi Denka Kogyo Co., Ltd.) is used. The thickness of the coating is about 2 to 20 μm, and can be set to a value having such a thickness that sufficient adhesive strength can be obtained and the transmittance is not lost. At this time, spacer particles, for example, 4 μm spherical particles (not shown) of benzoguanamine are mixed in the adhesive layer 60 as spacer means. The spacer particles are added in advance to the material to be applied, and are applied to the substrate 10. At this time, the adhesive is liquid, and it is desirable to control the thickness of the coating film slightly thicker than the size of the spacer particles. When the glass substrate 10 and the sheet base material 80 which is a plastic sheet are laminated in this state, the adhesive layer 60 having a uniform film thickness can be obtained. The amount of spacer particles mixed is preferably adjusted so that the in-plane distribution amount becomes about 40 particles / mm 2 after the adhesive layer 60 is formed. Here, the epoxy resin of the adhesive layer 60 causes volume shrinkage of, for example, about several percent by photocuring, but the spacer particles are unlikely to undergo such changes. Therefore, in accordance with the volume shrinkage of the adhesive layer 60, an undesirable deformation or stress occurs in the spacer particle portion, and a crack may occur in the ITO film. In order to avoid this, the particle diameter of the spacer particles should be a predetermined size or less, and is preferably set to 5.5 μm or less, for example. As the spacer means, in addition to the spacer particles, as shown in FIG. 6, between the color patterns 50Y, 50M, and 50C of the color filter layer 50 (this portion is also a portion without the pattern of the transparent conductive film 30), A spacer pattern 70 patterned in an island shape or a stripe shape can also be used. The spacer pattern 70 does not damage the transparent conductive film 30 due to undesired deformation or stress. The spacer pattern 70 can be formed using a polyimide resin mixed with a black color material. If it does so, when performing a liquid crystal display, the merit of improving the contrast of a display is also acquired.
[0016]
Thereafter, as shown in FIG. 7, a sheet base material 80 (having a thickness of 100 to 700 μm) made of a polyethersulfone substrate is disposed on the adhesive layer 60 side, and the transparent conductive film 30 and the color filter layer 50, etc. Is transferred from the glass substrate 10 side to the sheet base material 80 side. In this transfer process, ultraviolet rays are irradiated from the sheet base material 80 side. At the same time, the temperature increase on the side of the adhesive layer 60 (curing target) accompanying irradiation is actively suppressed, and the temperature is as close to room temperature as possible. To do. Since the transparent conductive film 30 that is particularly susceptible to damage during the transfer is sandwiched between the polyimide film 20 as the release layer and the protective film 40, it is effective from the external force accompanying the curing and transfer of the adhesive layer 60. Protected.
[0017]
After the transfer, the polyimide layer 20 as a release layer is removed. This is also to enable electrical connection between the transparent conductive film 30 and a driver IC for liquid crystal display, and to improve the effective voltage for driving the liquid crystal. For the removal of the polyimide layer 20, wet etching using hydrazine-ethylenediamine is used. At this time, the protective film 40 protects the adhesive layer 60 and the color filter layer 50 from the etchant.
[Brief description of the drawings]
FIG. 1 is a cross-sectional view showing a glass substrate on which a release layer is formed.
FIG. 2 is a cross-sectional view showing a state where a transparent conductive film is formed on a glass substrate.
FIG. 3 is a cross-sectional view showing a state in which a protective film is formed on a transparent conductive film pattern.
FIG. 4 is a cross-sectional view showing a state in which a color filter layer is formed on a protective film.
FIG. 5 is a cross-sectional view showing a state in which an adhesive layer is applied on a color filter layer.
FIG. 6 is a cross-sectional view when a spacer pattern is used.
FIG. 7 is a cross-sectional view showing a state during transfer.
[Explanation of symbols]
10 Glass substrate 20 Polyimide layer (peeling layer)
30 transparent conductive film 40 protective film 50 color filter layer 60 adhesive layer 70 spacer pattern 80 sheet base material

Claims (6)

プラスチック材料からなるシート基材の一面に、転写によって透明導電膜を形成するに際し、転写すべき前記透明導電膜を、前記プラスチック材料に比べて耐熱性にすぐれた基板側に形成しておく転写方法であって、前記透明導電膜は比抵抗３．０×１０ −４ Ωｃｍ以下の特性をもつものであり、前記耐熱性にすぐれた基板上に前記透明導電膜が、転写時に剥離部分となる剥離層と、その透明導電膜を保護するための保護膜とではさみ込まれ、それにより、クラックの発生が防止されていることを特徴とする、透明導電膜の転写方法。When forming a transparent conductive film by transfer on one surface of a sheet base material made of a plastic material, the transfer method is to form the transparent conductive film to be transferred on the substrate side that has better heat resistance than the plastic material The transparent conductive film has a characteristic of a specific resistance of 3.0 × 10 −4 Ωcm or less, and the transparent conductive film is peeled off on the substrate having excellent heat resistance as a peeling portion at the time of transfer. A method for transferring a transparent conductive film, characterized in that the layer is sandwiched between a protective film for protecting the transparent conductive film , thereby preventing generation of cracks . 前記耐熱性にすぐれた基板は、セラミックス、ガラス、金属の単体か、それらが複合された基板であり、しかも、前記剥離層は、ポリイミド系の樹脂からなる、請求項１の転写方法。The transfer method according to claim 1, wherein the substrate having excellent heat resistance is a single body of ceramic, glass, or metal, or a substrate in which these are combined, and the release layer is made of a polyimide resin. 前記耐熱性にすぐれた基板上、前記保護膜の上にさらに接着剤層を含む、請求項１の転写方法。The transfer method according to claim 1, further comprising an adhesive layer on the substrate having excellent heat resistance and on the protective film. 前記接着剤層の部分に、その接着剤層の厚さを制御するためのスペーサ手段を備える、請求項３の転写方法。The transfer method according to claim 3, further comprising spacer means for controlling a thickness of the adhesive layer in a portion of the adhesive layer. 前記スペーサ手段は、前記接着剤層の中に混入したスペーサ粒子、あるいは前記保護膜の上に形成したスペーサパターンのいずれかである、請求項４の転写方法。The transfer method according to claim 4, wherein the spacer means is either spacer particles mixed in the adhesive layer or a spacer pattern formed on the protective film. 前記透明導電膜は、液晶カラー表示装置の電極であり、カラー表示のためのカラーフィルタ層が前記保護膜の上に形成され、前記接着剤層がそのカラーフィルタ層を被っている、請求項３の転写方法。The transparent conductive film is an electrode of a liquid crystal color display device, a color filter layer for color display is formed on the protective film, and the adhesive layer covers the color filter layer. Transfer method.
JP11031099A 1999-04-19 1999-04-19 Transfer method of transparent conductive film Expired - Fee Related JP3909791B2 (en)

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JP11031099A JP3909791B2 (en) 1999-04-19 1999-04-19 Transfer method of transparent conductive film
US09/548,952 US6413693B1 (en) 1999-04-19 2000-04-13 Method for transferring transparent conductive film
DE60040361T DE60040361D1 (en) 1999-04-19 2000-04-17 Method for transmitting a transparent, conductive film
EP00303238A EP1046945B1 (en) 1999-04-19 2000-04-17 Method for transferring transparent conductive film
TW089107242A TW514607B (en) 1999-04-19 2000-04-18 Method for transferring transparent conductive film
KR10-2000-0020243A KR100382824B1 (en) 1999-04-19 2000-04-18 Method for transferring transparent conductive film
US10/027,289 US6830864B2 (en) 1999-04-19 2001-12-20 Method for transferring transparent conductive film

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